Silk is generally defined as protein polymers spun into fibers by some Lepidoptera larvae such as silk worms and spiders. Silk is an intriguing biomaterial because of its light weight, incredible strength, and elasticity. The major components of silkworm Bombyx mori silk are fibroin protein and glue-like sericin protein. Silk fibroin protein compositions are attractive in biomedical applications, such as tissue engineering, because of their biocompatibility, slow degradability, and excellent mechanical properties. Degradable silk fibroin formulations offer mechanically robust materials for a wide range of mechanical and functional properties for biomedical applications including drug delivery. Among the useful silk fibroin preparations are silk gels. There remains a need for additional approaches to forming silk gels for a variety of applications.